ACS ES&T Engineering
·
2023
·
IF 7.1
Beiping Zhang,Chaoting Guan,Qin Guo,Run Huang,Jin Jiang
Electrochemical technologies and permanganate oxidation are two attractive strategies in water treatment due to their low cost, easy operation, good adaptability, and environmental friendliness. Interestingly, recent studies have demonstrated that the combination of electrolysis and Mn(VII) (E-Mn(VII) process) shows a synergetic effect on organic contaminants degradation. However, the underlying mechanism of the E-Mn(VII) process remains unclear. In this study, the enhanced removal of diclofenac (DCF) by the E-Mn(VII) process was also demonstrated, and the main reactive species were reidentified. It was found that H2O2 was considerably formed via the reduction of O2 on the cathode, and it played a key role in facilitating Mn(VII) transformation into MnO2. Increasing O2 concentration, working potential, and pH value were conducive to H2O2 formation as well as Mn(VII) transformation to MnO2. Higher Mn(VII) dosages did not impact H2O2 formation but also led to faster MnO2 formation. The enhanced formation of MnO2 was favorable for the fast degradation of DCF in the E-Mn(VII) process owing to the catalytic effect of MnO2 on Mn(VII) oxidation. This was confirmed by the observation that (i) the E-Mn(VII) process showed a similar pH-dependent oxidation trend to that of MnO2 catalytic oxidation of Mn(VII) (i.e., the reactivity was much stronger at lower pH); and (ii) the addition of MnO2 prepared ex situ had a significant enhancing effect on DCF oxidation by the E-Mn(VII) process. Moreover, the possible contribution of reactive manganese intermediates such as soluble free Mn(III), Mn(VI), and Mn(V) was ruled out by the results of the probe experiments, UV–visible spectrophotometry, and examining the reactivity of Mn(III) complexes prepared ex situ. Also, the results of radical scavenging experiments indicated the negligible contribution of HO•. Furthermore, for the practical application of the E-Mn(VII) process in water decontamination, suitable operating parameters (e.g., a moderate potential and relatively lower pH) should be determined to avoid the fast loss of Mn(VII) and the electrical energy consumption. Overall, this work brings new insights into the reaction mechanism of the E-Mn(VII) process as well as proposes an efficient, sustainable, and feasible strategy for water and wastewater treatment.
研究领域:
环境科学
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化学工程
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水处理
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电化学
✓ 已验证
产品关联
DOI
高影响因子
MOLECULES
·
2023
·Vol. 28
·期 9
·3736
·
IF 4.6
Gege Yang,Ying Chen,Rui Shi,Rongrong Chen,Shanshan Gao,Xin Zhang,Yuan Rao,Ying Lu,Yuancheng Peng,Zhihe Qing,Chunxia Song
Platinum nanoparticles (PtNPs) are classical peroxidase-like nanozyme; self-agglomeration of nanoparticles leads to the undesirable reduction in stability and catalytic activity. Herein, a hybrid peroxidase-like nanocatalyst consisting of PtNPs in situ growing on g–C3N4nanosheets with enhanced peroxidase-mimic catalytic activity ([email protected]–C3N4nanosheets) was prepared for H2O2and oxidase-based colorimetric assay. g–C3N4nanosheets can be used as carriers to solve the problem of poor stability of PtNPs. We observed that the catalytic ability could be maintained for more than 90 days.[email protected]–C3N4nanosheets could quickly catalyze the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB), and the absorbance of blue color oxidized TMB (oxTMB) showed a robust linear relationship with the concentration of H2O2(the detection limit (LOD): 3.33 μM). By utilizing H2O2as a mediator, this strategy can be applied to oxidase-based biomolecules (glucose, organophosphorus, and so on, that generate or consume hydrogen peroxide) sensing. As a proof of concept, a sensitive assay of cholesterol that combined[email protected]–C3N4nanosheets with cholesterol oxidase (ChOx) cascade catalytic reaction was constructed with an LOD of 9.35 μM in a widespread range from 10 to 800 μM (R2= 0.9981). In addition, we also verified its ability to detect cholesterol in fetal bovine serum. These results showed application prospect of[email protected]–C3N4nanosheets-based colorimetry in sensing and clinical medical detection.Keywords:[email protected]–C3N4nanosheets;peroxidase-mimic;H2O2;oxidase-based sensing
研究领域:
纳米技术
·
分析化学
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生物传感器
·
医学诊断
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Frontiers in Bioengineering and Biotechnology
·
2023
·
IF 5.7
Yujia Liang,Zhengmin Cai,Yamei Tang,Chenglin Su,Liye Xie,Yan Li,Xinqiang Liang
Introduction: Reactive oxygen species (ROS)-mediated therapies have typically been considered as noninvasive tumor treatments owing to their high selectivity and efficiency. However, the harsh tumor microenvironment severely impairs their efficiency. Methods: Herein, the biodegradable Cu-doped zeolitic imidazolate framework-8 (ZIF-8) was synthesized for loading photosensitizer Chlorin e6 (Ce6) and CaO 2 nanoparticles, followed by surface decoration by hyaluronic acid (HA), obtaining HA/CaO 2 -Ce6@Cu-ZIF nano platform. Results and Discussion: Once HA/CaO 2 -Ce6@Cu-ZIF targets tumor sites, the degradation of Ce6 and CaO 2 release from the HA/CaO 2 -Ce6@Cu-ZIF in response to the acid environment, while the Cu 2+ active sites on Cu-ZIF are exposed. The released CaO 2 decompose to generate hydrogen peroxide (H 2 O 2 ) and oxygen (O 2 ), which alleviate the insufficiency of intracellular H 2 O 2 and hypoxia in tumor microenvironment (TME), effectively enhancing the production of hydroxyl radical (•OH) and singlet oxygen ( 1 O 2 ) in Cu 2+ -mediated chemodynamic therapy (CDT) and Ce6-induced photodynamic therapy (PDT), respectively. Importantly, Ca 2+ originating from CaO 2 could further enhance oxidative stress and result in mitochondrial dysfunction induced by Ca 2+ overloading. Conclusion: Thus, the H 2 O 2 /O 2 self-supplying and Ca 2+ overloading ZIF-based nanoplatform for cascade-amplified CDT/PDT synergistic strategy is promising for highly efficient anticancer therapy.
研究领域:
纳米技术
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癌症治疗
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材料科学
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生物医学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2020
·
IF 6.182
Wei Luo,Yi Liu,Fan Li,Jinghao Huo,Dan Zhao,Jianfeng Zhu,Shouwu Guo
The novel V 2 CT x MXenes have gained increasing attention as anode materials in lithium-ion batteries, but to boost their practical to the theoretical values is still challenging. Herein, the partially etched V 2 CT x was oxidized in the presence of H 2 O 2 through a hydrothermal reaction and the electrochemical properties of as-obtained oxidized V 2 CT x were assessed. It is illustrated that the oxidized V 2 CT x possesses a large surface interlayer spacing, and enriched with VO 2 (A) and O-terminate groups. Once used as anode materials for Li-ion batteries, the oxidized V 2 CT x shows enhanced specific lithium ion storage capacities of 318 mAh·g −1 at 100 mA·g −1 after 100 cycles, and 125 mAh·g −1 at 1000 mA·g −1 after 1000 cycles, and better cycling stability and excellent rate performance over the V 2 CT x .
研究领域:
材料科学
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电化学
·
能量存储
✓ 已验证
产品关联
DOI
高影响因子
BIOSENSORS & BIOELECTRONICS
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2016
·
IF 7.476
Liyan Zhang,Shuai Li,Minmin Dong,Yao Jiang,Ru Li,Shuo Zhang,Xiaoxia Lv,Lijun Chen,Hua Wang
A facile and efficient enzymatic reconstitution methodology has been proposed for high-catalysis peroxidase mimics by remolding the redox active centers of heme-containing proteins with the in-site biomineralized gold using hemoglobin (Hb) as a model. Catalytic hemin (Hem) was extracted from the active centers of Hb for the gold biomineralization and then reconstituted into apoHb to yield the Hem-Au@apoHb nanocomposites showing dramatically improved intrinsic catalysis and electrocatalysis over natural Hb and Hem. The biomineralized gold, on the one hand, would act as “nanowires” to promote the electron transferring of the nanocomposites. On the other hand, it would create a reactivity pathway to pre-organize and accumulate more substrates towards the active sites of the peroxidase mimics. Steady-state kinetics studies indicate that Hem-Au@apoHb could present much higher substrate affinity (lower Michaelis constants) and intrinsic catalysis even than some natural peroxidases. Moreover, the application feasibility of the prepared artificial enzymes was demonstrated by colorimetric assays and direct electrocatalysis for H 2 O 2 sensing, showing a detection limitation low as 0.45 μM. Importantly, such a catalysis active-center reconstitution protocol may circumvent the substantial improvement of the intrinsic catalysis and electrocatalysis of diverse heme-containing proteins or enyzmes toward the extensive applications in the chemical, enviromental, and biomedical catalysis fields.
研究领域:
生物化学
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纳米生物学
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酶工程
·
分析化学
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Yuanhong Xie,Chenrui Liu,Dejian Li,Yun Liu
Herein, a novel composite of MIL-101(Fe) loaded with nitrogen doped carbon quantum dots (NCQDs/MIL-101(Fe), denoted as NQML), which can construct dual effect of photocatalysis and photo-Fenton for organic pollutants removal, was prepared by solvent impregnation method. Characterization methods proved that NQML had been synthesized successfully. Additionally, the adding volume of NCQDs could effectively influence the photocatalytic activities of NQML-x composites (x represents the adding volume of NCQDs) for tetracycline (TC) degradation, and NQML-8 exhibited the optimum photocatalytic performance among the studied catalysts upon visible light illumination under natural pH, which can completely degrade TC within 180 min. By comparison, the TC degradation kinetic constant in the system with NQML-8 was as 15.85 and 8.24 folds of that in the NCQDs and MIL-101(Fe) systems, respectively. The mechanism study proved that the enhanced photocatalytic performance of NQML was resulted from the visible light up-conversion property, electron-hole separation and transfer capacity of NCQDs. Meanwhile, NQML could not only produce h + but also lead to in-situ generation of O 2 - and H 2 O 2 by activation of O 2 under visible light. The generated H 2 O 2 could react with Fe(II) in MIL-101(Fe) to produce OH so as to construct a dual effect of photocatalysis and photo-Fenton in TC removal.
研究领域:
环境科学
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材料科学
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化学工程
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光化学
✓ 已验证
产品关联
DOI
高影响因子
ELECTROANALYSIS
·
2017
·Vol. 29
·期 9
·2044-2052
·
IF 2.851
Yongqin Liu,Lu Wang,Lingxi Yang,Yi Zhan,Lina Zou,Baoxian Ye
This paper demonstrated using polyethylenimine (PEI)-functionalized graphene (Gr) incorporating tin oxide (SnO 2 ) hybrid nanocomposite as a platform for nonenzymatic H 2 O 2 electrochemical sensor. The results of UV-vis spectroscopy and X-ray diffraction (XRD) confirmed the simultaneous formation of tin oxide (SnO 2 ) nanocomposite and reduction of graphene oxide (GO). Transmission electron microscopy (TEM) images showed a uniform distribution of nanometer-sized tin oxide nanoparticles on the grapheme sheets, which could be achieved using stannous chloride (SnCl 2 ) complex instead of tin oxide as precursor. The electrochemical measurements, including cyclic voltammetry (CV) and amperometric performance (I-t), showed that the PEI-functionalized Gr supported SnO 2 (SnO 2 -PEI-Gr) exhibited an excellent electrocatalytic activity toward the H 2 O 2 . The corresponding calibration curve of the current response showed a linear detection range of 9×10 −6 ∼1.64×10 −3 mol L −1 , while the limit of detection was estimated to be 1×10 −6 mol L −1 . Electrochemical studies indicated that SnO 2 and functionalized Gr worked synergistically for the detection of H 2 O 2 .
研究领域:
电化学
·
纳米材料
·
传感器
✓ 已验证
产品关联
DOI
高影响因子
BIOMATERIALS
·
2021
·
IF 12.479
Jichun Yang,Shuojiong Pan,Shiqian Gao,Tianyu Li,Huaping Xu
Carbon monoxide (CO) therapy and antiangiogenesis therapy (AAT) are regarded as promising approaches for cancer treatment. However, the poor tumor targeting ability and inevitable side effects prevent their clinical application. In this study, we developed H 2 O 2 -responsive diselenide-containing micelles that combined CO therapy with chemosensitization therapy and AAT in a single system. Under the interaction of intratumoral H 2 O 2 , CO and gemcitabine (GEM) were released in situ from the micelles to reduce side effects, and CO significantly sensitized the chemotherapeutic effect of GEM by elevating the level of reactive oxygen species (ROS) in human gastric cancer AGS cells. Furthermore, diselenide bonds in the micelles were oxidized to seleninic acid in organic form, which suppressed the expressions of vascular endothelial growth factor (VEGF) and matrix metalloproteinase-2 (MMP-2) to realize AAT. This study provides an integrated solution to combine CO therapy with chemosensitization therapy and AAT together with good biocompatibility .
研究领域:
癌症治疗
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药学
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材料科学
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生物医学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Acta Biomaterialia
·
2021
·
IF 8.947
Chao-Qing Li,Meng-Wen Ma,Bin Zhang,Wei Chen,Zhong-Yuan Yin,Xiao-Ting Xie,Xiao-Lin Hou,Yuan-Di Zhao,Bo Liu
A nanoplatform based on Ag 2 S quantum dots (QDs) and tellurium nanorods (TeNRs) was developed for combined chemo-photothermal therapy guided by H 2 O 2 -activated near-infrared (NIR)-II fluorescence imaging. Polypeptide PC 10 AGRD-modified TeNRs and Ag 2 S QDs were co-encapsulated in 4T1 cell membrane to prepare a nanoplatform ( [email protected] ). Ag 2 S QDs and TeNRs in the [email protected] were used as a fluorescence probe and photosensitizer , and a chemotherapeutic prodrug and quenching agent to quench the fluorescence of Ag 2 S QDs, respectively. After the [email protected] was specifically targeted to the tumor site, the TeNRs were dissolved by the high concentration of H 2 O 2 at the tumor site to light up the fluorescence of Ag 2 S QDs for NIR-II fluorescence imaging. In addition, the generated toxic TeO 6 6− molecules decreased ATP production by selective cancer chemotherapy, which is beneficial for photothermal therapy. The elevated temperature due to photothermal therapy in turn promoted the chemical reaction in chemotherapy. In vitro and in vivo toxicity results showed that the [email protected] possesses high biocompatibility. Compared to single photothermal therapy and chemotherapy, the synergistic chemo-photothermal therapy can effectively suppress the growth of 4T1 tumor. This all-in-one nanoplatform provides a boulevard for the combination therapy of tumors guided by NIR-II fluorescence imaging. Statement of significance NIR-II fluorescence imaging shows the characteristics of low tissue absorption, reflection, and scattering, which can greatly reduce the influence of autofluorescence in vivo . However, the non-negligible effect of autofluorescence is still observed in fluorescence imaging in vivo . Therefore, there is an urgent need to develop a strategy of controlled release of fluorescence for accurate imaging and tumor therapy. Here, Ag 2 S quantum dots (QDs) with NIR-II fluorescence emission and good photothermal conversion efficiency are used as a fluorescence probe and photosensitizer, and tellurium nanorods (TeNRs) are used as a chemotherapeutic prodrug and quenching agent to quench the fluorescence of Ag 2 S QDs. This multiple nanoplatform provides an inspiration for the combination therapy of tumor guided by NIR-II fluorescence imaging.
研究领域:
生物医学工程
·
肿瘤学
·
纳米医学
·
影像医学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Water Process Engineering
·
2025
·
IF 6.7
Xiang Gong,Suqi Li,Xiulan Guo,Jiaqiao Yuan,Hongyu Lu,Shuming Wen,Pan Yu,Shaojun Bai,Dandan Wu
This work investigates the efficiency removal and mechanism of xanthate from flotation tailings wastewater through a coagulation-Fenton oxidation process by introducing Fe 2+ and Mn 2+ to activate H 2 O 2 . Under the conditions of initial 60 mg/L SBX concentration, 50 mg/L H 2 O 2 concentration, 25 mg/L Fe 2+ concentration, 25 mg/L Mn 2+ concentration, 3.5 initial pH, and 60 min reaction time, the degradation rate of xanthate was more than 98 %. The H 2 O 2 + Fe 2+ +Mn 2+ system exhibits markedly superior degradation efficiency for SBX. The results demonstrate that the Fe 2+ +Mn 2+ bimetallic system in simulated AMD facilitates the activation of H 2 O 2 to generate a greater abundance of hydroxyl radicals (•OH). Through characterization of degradation products and analysis of intermediates, two potential degradation pathways of SBX are proposed. In the first pathway, SBX initially undergoes conversion to BPX, which subsequently degrades into small molecular compounds including CO 2 , H 2 O, and SO 4 2− under sustained •OH radical attack. The secondary pathway involves the formation of precipitates composed of xanthates metal (Fe/Mn), iron oxides, and manganese oxides. This work presents a new strategy for efficiently degrading xanthate contaminants in mineral flotation wastewater. It also valorizes AMD by exploiting its intrinsic properties, thereby mitigating AMD's environmental hazards at the source.
研究领域:
环境工程
·
化学工程
·
矿物加工
·
废水处理
·
高级氧化工艺
✓ 已验证
产品关联
DOI
高影响因子
ULTRASONICS SONOCHEMISTRY
·
2024
·
IF 8.7
Yunxiang Que,Yao Zhang,Fengxiang Liang,Liping Wang,Yiting Yang,Jingbo Zhang,Wanting Wang,Ying Sun,Changjiao Zhong,Haipeng Zhang,Chengguang He,Lili Guan,Hongxia Ma
Adhere to the concept of low-carbon environmental protection and turning waste into treasure, polysaccharides from Flammulina velutipes residue polysaccharide (FVRP) has been developed and possesses diverse bioactivities, comprising antioxidant, hypoglycemic, and relieving heavy metal damage, which still has the disadvantages of high molecular weight and low bioavailability. The current work is the first to prepare a degraded polysaccharide (FVRPV) from FVRP by ultrasonic assisted H 2 O 2 -Vc technique in order to reduce its molecular weight, thereby improving its activity and bioavailability. Our results found that the molecular weight and average particle size were declined, but the monosaccharide composition and characteristic functional group types of FVRPV had no impact. The structural changes of polysaccharides analyzed by XRD, Congo Red test, I 2 -KI, SEM, and methylation analysis indicated that the surface morphology and glycosidic bond composition of FVRPV possessed longer side chains and a greater number of branches with an amorphous crystal structure devoid of a triple helix configuration, and had experienced notable alterations after ultrasonic assisted H 2 O 2 -Vc treatment. Meanwhile, the in vitro antioxidant capacity of FVRPV had significantly increased compared to FVRP, implying ultrasonic assisted H 2 O 2 -Vc technique maybe a effective method to enhance the bioactivity of polysaccharides. In addition, the content of polysaccharide, reducing sugar, and uronic acid in FVRPV was significantly decreased, but antioxidant capacity of fermentation broth was stronger by in vitro human fecal fermentation. The 16S rDNA sequencing data displayed that FVRPV can enrich probiotics and reduce the abundance of pathogenic bacteria through different metabolic pathways mediated by gut microbiota, thereby exerting its potential probiotic effects. The interesting work provides a novel degraded polysaccharide by ultrasonic assisted H 2 O 2 -Vc technique, laying a foundation for developing FVRPV as a new antioxidant and prebiotic.
研究领域:
食品科学
·
生物技术
·
生物化学
·
微生物学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Catalysis
·
2024
·
IF 11.3
Jiayu An,Wenjun Jiang,Fuwei Zhuang,Yinhua Ma,Su Zhan,Feng Zhou
Utilizing photocatalytic technology to achieve efficient production of H2O2 is a hot topic. Here, we synthesized a photocatalytic material with a strong built-in electric field, namely, Pym-CN, through a hydrothermal-assisted thermal polymerization strategy, which effectively promotes the separation and transfer of photoinduced charge carriers. A pyrimidine ring was successfully introduced into the heptazine structure unit of Pym-CN, which leads to electron aggregation at N═C–N, benefiting for enhancing the strong sorption and activation capabilities of oxygen. Under the condition of visible light wavelength greater than 400 nm (λ > 400 nm), the H2O2 production rate of Pym-CN (2622.5 μmol/L/h) is 7.6 times that of the BCN. A detailed investigation of the reaction mechanism revealed that Pym-CN follows a two-step continuous process of single-electron oxygen reduction reaction (ORR). This work elucidates the application prospects of the donor–acceptor (D–A) structure with a strong built-in electric field in the field of efficient photocatalytic production of H2O2.
研究领域:
材料科学
·
光催化
·
可再生能源
·
化学工程
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）